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A new solid-contact ion-selective electrode (ISE) sensitive to lead (II) ions, obtained by modifying a polymer membrane with a nanocomposite of carbon nanofibers and an ionic liquid 1-hexyl-3-methylimidazolium hexafluorophosphate, is presented. Electrodes with a different amount of nanocomposite in the membrane (0–9% w/w), in which a platinum wire or a glassy carbon electrode was used as an internal electrode, were tested. Potentiometric and electrochemical impedance spectroscopy measurements were carried out to determine the effect of the ion-sensitive membrane modification on the analytical and electrical parameters of the ion-selective electrode. It was found that the addition of the nanocomposite causes beneficial changes in the properties of the membrane, i.e., a decrease in resistance and an increase in capacitance and hydrophobicity. As a result, the electrodes with the modified membrane were characterized by a lower limit of detection, a wider measuring range and better selectivity compared to the unmodified electrode. Moreover, a significant improvement in the stability and reversibility of the electrode potential was observed, and additionally, they were resistant to changes in the redox potential of the sample. The best parameters were shown by the electrode obtained with the use of a platinum wire as the inner electrode with a membrane containing 6% of the nanocomposite. The electrode exhibited a Nernstian response to lead ions over a wide concentration range, 1.0 × 10−8–1.0 × 10−2 mol L−1, with a slope of 31.5 mV/decade and detection limit of 6.0 × 10−9 mol L−1. In addition, the proposed sensor showed very good long term stability and worked properly 4 months after its preparation without essential changes in the E0 or slope values. It was used to analyze a real sample and correct results of lead content determination were obtained. [ABSTRACT FROM AUTHOR]